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1.
Nat Commun ; 13(1): 6146, 2022 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-36253383

RESUMO

Selective C-H bond activation is one of the most challenging topics for organic reactions. The difficulties arise not only from the high C-H bond dissociation enthalpies but also the existence of multiple equivalent/quasi-equivalent reaction sites in organic molecules. Here, we successfully achieve the selective activation of four quasi-equivalent C-H bonds in a specially designed nitrogen-containing polycyclic hydrocarbon (N-PH). Density functional theory calculations reveal that the adsorption of N-PH on Ag(100) differentiates the activity of the four ortho C(sp3) atoms in the N-heterocycles into two groups, suggesting a selective dehydrogenation, which is demonstrated by sequential-annealing experiments of N-PH/Ag(100). Further annealing leads to the formation of N-doped graphene nanoribbons with partial corannulene motifs, realized by the C-H bond activation process. Our work provides a route of designing precursor molecules with ortho C(sp3) atom in an N-heterocycle to realize surface-induced selective dehydrogenation in quasi-equivalent sites.

2.
J Phys Condens Matter ; 33(22)2021 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-33596556

RESUMO

Two-dimensional (2D) Dirac materials have attracted intense research efforts due to their promise for applications ranging from field-effect transistors and low-power electronics to fault-tolerant quantum computation. One key challenge is to fabricate 2D Dirac materials hosting Dirac electrons. Here, monolayer germanene is successfully fabricated on a Ag2Ge surface alloy. Scanning tunneling spectroscopy measurements revealed a linear energy dispersion relation. The latter was supported by density functional theory calculations. These results demonstrate that monolayer germanene can be realistically fabricated on a Ag2Ge surface alloy. The finding opens the door to exploration and study of 2D Dirac material physics and device applications.

3.
ACS Nano ; 15(3): 4481-4489, 2021 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-33656862

RESUMO

As a two-dimensional semiconductor with many physical properties, including, notably, layer-controlled electronic bandgap and coupled spin-valley degree of freedom, monolayer MoSe2 is a strong candidate material for next-generation opto- and valley-electronic devices. However, due to substrate effects such as lattice mismatch and dielectric screening, preserving the monolayer's intrinsic properties remains challenging. This issue is generally significant for metallic substrates whose active surfaces are commonly utilized to achieve direct chemical or physical vapor growth of the monolayer films. Here, we demonstrate high-temperature-annealed Au foil with well-defined (100) facets as a weakly interacting substrate for atmospheric pressure chemical vapor deposition of highly crystalline monolayer MoSe2. Low-temperature scanning tunneling microscopy/spectroscopy measurements reveal a honeycomb structure of MoSe2 with a quasi-particle bandgap of 1.96 eV, a value comparable with other weakly interacting systems such as MoSe2/graphite. Density functional theory calculations indicate that the Au(100) surface exhibits the preferred energetics to electronically decouple from MoSe2, compared with the (110) and (111) crystal planes. This weak coupling is critical for the easy transfer of monolayers to another host substrate. Our study demonstrates a practical means to produce high-quality monolayers of transition-metal dichalcogenides, viable for both fundamental and application studies.

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